Wafer-scale Hybrid Molecular Beam Epitaxy of BaTiO ₃ and SrTiO ₃ on Silicon

The integration of epitaxial barium titanate (BTO) on silicon represents a highly promising pathway for next-generation, energy-efficient photonic integrated circuits due to BTO’s exceptionally high Pockels coefficients. However, the scalable epitaxy of BTO on Si remains challenged by complicated stoichiometry control and slow growth rates. In this work, we demonstrate the continuous, wafer-scale growth of high-quality BTO films on SrTiO3 (STO)-buffered 4-inch Si (001) wafers using a fully hybrid molecular beam epitaxy (hMBE) approach. By utilizing titanium tetraisopropoxide as a titanium precursor, we achieve a self-regulating, adsorption-controlled layer-by-layer growth at rates exceeding 75 nm·h−1, while maintaining an atomically sharp and structurally coherent BTO/STO interface. We systematically compare the structural, ferroelectric, and electro-optic (EO) properties of fully hMBE-grown BTO with those deposited via pulsed laser deposition (PLD) on identical STO/Si templates. While both techniques yield high-quality c-domain dominated films, the optimized hMBE-grown BTO exhibits superior crystallinity and a larger effective EO coefficient of 248 pm·V−1, surpassing that of the PLD-grown films (220 pm·V−1), in addition to an elevated Curie temperature of above 200 °C. These results highlight the advantages of the fully hMBE approach as a scalable, deterministic, and high-performance materials platform for wafer-scale integrated ferroelectric photonics.